Tracking the local order parameter through the Hubbard exciton decoherence time in the Mott-Hubbard insulator LaVO3

Abstract

The prototypical Mott-Hubbard insulator LaVO3 undergoes a structural phase transition accompanied by the onset of spin and orbital ordering below 140 K. By combining ultrafast optical pump-probe spectroscopy and two-dimensional electronic spectroscopy, we investigate the interplay between fluctuations of the local spin and orbital order parameter and the lifetime of high-energy electron-hole excitations. Specifically, we demonstrate that the pump-induced perturbation of the order parameter leads to a change of the Hubbard exciton decoherence time and, consequently, of its homogeneous linewidth. Dynamical mean-field theory calculations confirm that the exciton scattering rate is crucially affected by the degree of order of the spin and orbital lattices in LaVO3. Our results demonstrate that multi-dimensional ultrafast optical spectroscopy can be used to track the dynamics of the order parameter, thus opening new routes in the study of correlated quantum materials characterized by intertwined orders.